Ordered graphane nanoribbons synthesized via high-pressure diels-alder polymerization of 2,2'-bipyrazine

Li, F.*; Tang, X.*; Fei, Y.*; Zhang, J.*; Liu, J.*; Lang, P.*; Che, G.*; Zhao, Z.*; Zheng, Y.*; Fang, Y.*; et al.

Journal of the American Chemical Society, 147(17), p.14054 - 14059, 2025/04

https://doi.org/10.1021/jacs.5c03116

We synthesized a crystalline graphane nanoribbon (GANR) via pressure-induced polymerization of 2,2'-bipyrazine (BPZ). By performing Rietveld refinement of in situ neutron diffraction data, nuclear magnetic resonance spectroscopy, infrared spectra, and theoretical calculation, we found that BPZ experienced Diels-Alder polymerization between the stacked aromatic rings, and formed extended boat-GANR structures with exceptional long-range order. The unreacted -C=N- groups bridge the two ends of the boat, and ready for further functionalization. The GANR has a bandgap of 2.25 eV, with booming photoelectric response (/ =18.8). Our work highlights that the high-pressure topochemical polymerization is a promising method for the precise synthesis of graphane with specific structure and desired properties.

Uncertainty quantification for severe-accident reactor modelling; Results and conclusions of the MUSA reactor applications work package

Brumm, S.*; Gabrielli, F.*; Sanchez Espinoza, V.*; Stakhanova, A.*; Groudev, P.*; Petrova, P.*; Vryashkova, P.*; Ou, P.*; Zhang, W.*; Malkhasyan, A.*; et al.

Annals of Nuclear Energy, 211, p.110962_1 - 110962_16, 2025/02

https://doi.org/10.1016/j.anucene.2024.110962

High-pressure polymerization of phenol toward degree-4 carbon nanothread

Yang, X.*; Che, G.*; Wang, Y.*; Zhang, P.*; Tang, X.*; Lang, P.*; Gao, D.*; Wang, X.*; Wang, Y.*; Hattori, Takanori; et al.

Nano Letters, 25(3), p.1028 - 1035, 2025/01

https://doi.org/10.1021/acs.nanolett.4c04895

Saturated sp-carbon nanothreads (CNTh) have garnered significant interest due to their predicted high Young's modulus and thermal conductivity. While the incorporation of heteroatoms into the central ring has been shown to influence the formation of CNTh and yield chemically homogeneous products, the impact of pendant groups on the polymerization process remains underexplored. In this study, we investigate the pressure-induced polymerization of phenol, revealing two phase transitions occurring below 0.5 and 4 GPa. Above 20 GPa, phenol polymerizes into degree-4 CNThs featuring hydroxyl and carbonyl groups. Hydrogen transfer of hydroxyl groups was found to hinder the formation of degree-6 nanothreads. Our findings highlight the crucial role of the hydroxyl group in halting further intracolumn polymerization and offer valuable insights for future mechanism research and nanomaterial synthesis.

Solid-state Alder-ene reaction of 1-hexene under high pressure

Xu, J.*; Lang, P.*; Liang, S.*; Zhang, J.*; Fei, Y.*; Wang, Y.*; Gao, D.*; Hattori, Takanori; Abe, Jun*; Dong, X.*; et al.

Journal of Physical Chemistry Letters (Internet), p.2445 - 2451, 2025/00

https://doi.org/10.1021/acs.jpclett.4c03696

The Alder-ene reaction is a chemical reaction between an alkene with an allylic hydrogen, and it provides an efficient method to construct the C-C bond. Traditionally, this reaction requires catalysts, high temperatures, or photocatalysis. In this study, we reported a high-pressure-induced solid-state Alder-ene reaction of 1-hexene at room temperature without a catalyst. 1-Hexene crystallizes at 4.3 GPa and polymerizes at 18 GPa, forming olefins. By exploring gas chromatography-mass spectrometry, we discovered that 1-hexene generates dimeric products through the Alder-ene reaction under high pressures. The in situ neutron diffraction shows that the reaction process did not obey the topochemical rule. A six-membered ring transition state including one C-H bond and two alkene bonds was evidenced by the theoretical calculation, whose energy obviously decreased when compressed to 20 GPa. Our work offers a novel and promising method to realize the Alder-ene reaction at room temperature without a catalyst, expanding the application of this important reaction.

Strong low-energy rattling modes enabled liquid-like ultralow thermal conductivity in a well-ordered solid

Liu, P.-F.*; Li, X.*; Li, J.*; Zhu, J.*; Tong, Z.*; Kofu, Maiko*; Nirei, Masami; Xu, J.*; Yin, W.*; Wang, F.*; et al.

National Science Review, 11(12), p.nwae216_1 - nwae216_10, 2024/12

https://doi.org/10.1093/nsr/nwae216

Brightening triplet excitons enable high-performance white-light emission in organic small molecules via integrating n-- transitions

Yang, Q.*; Yang, X.*; Wang, Y.*; Fei, Y.*; Li, F.*; Zheng, H.*; Li, K.*; Han, Y.*; Hattori, Takanori; Zhu, P.*; et al.

Nature Communications (Internet), 15, p.7778_1 - 7778_9, 2024/09

https://doi.org/10.1038/s41467-024-52196-7

Luminescent materials that simultaneously embody bright singlet and triplet excitons hold great potential in optoelectronics, signage, and information encryption. However, achieving high-performance white-light emission is severely hampered by their inherent unbalanced contribution of fluorescence and phosphorescence. Herein, we address this challenge by pressure treatment engineering via hydrogen bonding cooperativity effect to realize the mixture of n-- transitions, where the triplet state emission was boosted from 7% to 40% in isophthalic acid (IPA). A superior white-light emission based on hybrid fluorescence and phosphorescence was harvested in pressure-treated IPA, and the photoluminescence quantum yield was increased to 75% from the initial 19% (blue-light emission). In-situ high-pressure IR spectra, X ray diffraction, and neutron diffraction reveal continuous strengthening of the hydrogen bonds with the increase of pressure. Furthermore, this enhanced hydrogen bond is retained down to the ambient conditions after pressure treatment, awarding the targeted IPA efficient intersystem crossing for balanced singlet/triplet excitons population and resulting in efficient white-light emission. This work not only proposes a route for brightening triplet states in organic small molecule, but also regulates the ratio of singlet and triplet excitons to construct high-performance white-light emission.

Probabilistic fracture mechanics analyses of a reactor pressure vessel using the irradiation embrittlement evaluation based on the Bayesian nonparametric method

Takamizawa, Hisashi; Lu, K.*; Li, Y.

International Journal of Pressure Vessels and Piping, 210, p.105219_1 - 105219_7, 2024/08

https://doi.org/10.1016/j.ijpvp.2024.105219

In the structural integrity assessment of an embrittled reactor pressure vessel (RPV) based on probabilistic fracture mechanics (PFM), it is crucial to consider both of the mean value and the uncertainty of the embrittlement prediction. Typically, the embrittlement prediction uncertainty is given by a normal distribution, and its standard deviation is determined from the residuals of the measured and predicted values of all data used to develop the embrittlement prediction method. Therefore, the same uncertainty is assumed regardless of neutron fluence and the available data. To overcome this issue, the Japan Atomic Energy Agency recently developed the embrittlement prediction method based on machine learning and Bayesian statistics, i.e., the Bayesian nonparametric (BNP) method, and introduced it to the PFM analysis code. The BNP method can predict the probability distribution according to data scarcity and provide more reasonable uncertainty because it estimates significant uncertainties where the scatter of actual measured data is large and the number of data is small. In this study, PFM analysis for a Japanese model RPV in a pressurized water reactor is conducted using the PFM analysis of structural components in aging light water reactors, where the embrittlement probability distribution calculated using the BNP method is used. Furthermore, the effects of different embrittlement prediction methods and uncertainties on the failure frequency of RPVs are investigated in the PFM analyses, and the results are presented.

Gradient residual strain measurement procedure in surface impacted railway steel axles by using neutron scattering

Zhou, L.*; Zhang, H.*; Qin, T. Y.*; Hu, F. F.*; Xu, P. G.; Ao, N.*; Su, Y. H.; He, L. H.*; Li, X. H.*; Zhang, J. R.*; et al.

Metallurgical and Materials Transactions A, 55(7), p.2175 - 2185, 2024/07

https://doi.org/10.1007/s11661-024-07352-5

Investigating the influence of analysis parameters in three-dimensional elasto-plastic finite element analysis of a gate-type piping support structure

Takito, Kiyotaka; Okuda, Yukihiko; Nishida, Akemi; Li, Y.

Proceedings of ASME 2024 Pressure Vessels & Piping Conference (PVP 2024) (Internet), 9 Pages, 2024/07

In probabilistic risk assessment against earthquakes (seismic PRA), one of the important issues is the development of a realistic response analysis method for evaluating the fragility of equipment and piping systems subject to input ground motions exceeding design assumption. Particularly, piping systems have complex plant-specific three-dimensional geometries. The arrangement and rigidity of piping support structures have significant impact on the response characteristics of the entire piping system. Therefore, it is necessary to develop a seismic response analysis method for piping systems, including piping support structures. To this end, the authors have been working on the development of elasto-plastic analysis method for piping support structures in order to establish a realistic response analysis method for piping systems including piping support structures. In this study, parametric studies on important analytical parameters were conducted to understand the influence of the analytical parameters on the deformation in the elasto-plastic analysis of piping support structures. At first, a three-dimensional finite element analysis model was created for cyclic loading tests of a gate type piping support structure assuming large deformations. Using the model, parametric studies were conducted for analysis parameters such as yield stress, secondary stiffness and element size. As the result, the influences of the analysis parameters on the analysis results were quantitatively clarified, which provided insight into the methodology for setting appropriate analysis parameters on elasto-plastic analysis for piping support structures.

Analyses of stress intensity factor solutions for subsurface flaws in flat plates

Li, S.; Li, Y.; Lu, K.*; Lacroix, V.*; Dulieu, P.*

Proceedings of ASME 2024 Pressure Vessels & Piping Conference (PVP 2024) (Internet), 18 Pages, 2024/07

https://doi.org/10.1115/PVP2024-122733